, Volume 13, Issue 3–4, pp 385–397

Reversible chemisorption of carbon dioxide: simultaneous production of fuel-cell grade H2 and compressed CO2 from synthesis gas

  • K. B. Lee
  • M. G. Beaver
  • H. S. Caram
  • S. Sircar


One vision of clean energy for the future is to produce hydrogen from coal in an ultra-clean plant. The conventional route consists of reacting the coal gasification product (after removal of trace impurities) with steam in a water gas shift (WGS) reactor to convert CO to CO2 and H2, followed by purification of the effluent gas in a pressure swing adsorption (PSA) unit to produce a high purity hydrogen product. PSA processes can also be designed to produce a CO2 by-product at ambient pressure. This work proposes a novel concept called “Thermal Swing Sorption Enhanced Reaction (TSSER)” which simultaneously carries out the WGS reaction and the removal of CO2 from the reaction zone by using a CO2 chemisorbent in a single unit operation. The concept directly produces a fuel-cell grade H2 and compressed CO2 as a by-product gas. Removal of CO2 from the reaction zone circumvents the equilibrium limitations of the reversible WGS reaction and enhances its forward rate of reaction. Recently measured sorption-desorption characteristics of two novel, reversible CO2 chemisorbents (K2CO3 promoted hydrotalcite and Na2O promoted alumina) are reviewed and the simulated performance of the proposed TSSER concept using the promoted hydrotalcite as the chemisorbent is reported.


Thermal swing sorption enhanced reaction Chemisorption Hydrogen Carbon dioxide Promoted hydrotalcite Promoted alumina 


Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.


  1. Chakravarti, S., Gupta, A., Hunek, B.: Advanced technology for the capture of CO2 from flue gases, First National Conference on Carbon Sequestration, Washington, DC, May 15–17 (2001) Google Scholar
  2. Chue, K.T., Kim, J.N., Yoo, Y.J., Cho, S.H., Yang, R.T.: Comparison of activated carbon and zeolite 13X for CO2 recovery from flue gas by pressure swing adsorption. Ind. Eng. Chem. Res. 34, 591–598 (1995) CrossRefGoogle Scholar
  3. Ding, Y., Alpay, E.: Adsorption-enhanced steam-methane reforming. Chem. Eng. Sci. 55, 3929–3940 (2000) CrossRefGoogle Scholar
  4. Fuderer, A., Rudelstorfer, E.: Selective adsorption of gases. U.S. Patent No 3,986,849 (1976) Google Scholar
  5. Hufton, J.R., Mayorga, S., Sircar, S.: Sorption-enhanced reaction process for hydrogen production. AIChE J. 45, 248–256 (1999) CrossRefGoogle Scholar
  6. Hufton, J.R., Weigel, S.J., Waldron, W.F., Rao, M., Nataraj, S., Sircar, S., Gaffney, T.R.: Sorption enhanced reaction process for production of hydrogen. DOE Report DE-FC36-95G010059 (2000) Google Scholar
  7. IEA Greenhouse Gas R&D Programme: Carbon Dioxide Capture from Power Stations. Cheltenham, United Kingdom (1990) Google Scholar
  8. Karasaki, M., Iijima, M., Shigeaki, M.: Removal of CO2 from flue gases. Japanese Patent No 7,313,840 (1995) Google Scholar
  9. Koros, W.J., Chern, R.T.: Separation of gas mixtures using polymeric membranes. In: Rousseau, R.W. (ed.) Handbook of Separation Process Technology, pp. 862–953. Wiley InterScience, New York (1987) Google Scholar
  10. Leci, C.L., Goldthorpe, S.H.: Assessment of CO2 removal from power station flue gas. Energy Convers. Manag. 33, 477–485 (1992) CrossRefGoogle Scholar
  11. Lee, K.B., Beaver, M.G., Caram, H.S., Sircar, S.: Novel thermal swing sorption enhanced reaction process concept for hydrogen production by low temperature steam methane reforming. Ind. Eng. Chem. Res. 46, 5003–5014 (2007a) CrossRefGoogle Scholar
  12. Lee, K.B., Verdooren, A., Caram, H.S., Sircar, S.: Chemisorption of carbon dioxide on potassium-carbonate-promoted hydrotalcite. J. Colloid Interface Sci. 308, 30–39 (2007b) CrossRefGoogle Scholar
  13. Lee, K.B., Beaver, M.G., Caram, H.S., Sircar, S.: Chemisorption of carbon dioxide on sodium oxide promoted alumina. AIChE J. (2007c, in press) Google Scholar
  14. Levenspiel, O.: Chemical Reaction Engineering: An Introduction to the Design of Reactors. Wiley, New York (1962) Google Scholar
  15. Matsumoto, H., Kitamura, H., Kamata, T., Nishikawa, N., Ishibashi, M.: Fundamental study of CO2 removal from thermal power plant flue gas by hollow-fiber gas-liquid contactor. Kagaku Kogaku Ronbun. 18, 804–812 (1992) Google Scholar
  16. Mimura, T., Shimojo, S., Suda, T., Iijima, M., Mitsuoka, S.: Research and development on energy saving technology for flue gas carbon dioxide recovery and steam system in power plant. Energy Convers. Manag. 36, 397–400 (1995) CrossRefGoogle Scholar
  17. National Research Council and National Academy of Engineering: The Hydrogen Economy: Opportunities, Costs, Barriers, and R&D Needs. The National Academic Press, Washington (2004) Google Scholar
  18. Qunying, J., Sixun, L.: Method for continuously gasifying coal (coke) and purifying synthesis gas. Chinese Patent No 1,156,754 (1997) Google Scholar
  19. Rase, H.F.: Chemical Reactor Design for Process Plants. Wiley, New York (1977) Google Scholar
  20. Rosen, M.A., Scott, D.S.: An energy-exergy analysis of the Koppers-Totzek process for producing hydrogen from coal. Int. J. Hydrogen Energ. 12, 837–845 (1987) CrossRefGoogle Scholar
  21. Schlinger, W.G., Kolaian, J.H., Quintana, M.E., Dorawala, T.G.: Texaco coal gasification process for production of clean synthesis gas from coke. Energy Prog. 5, 234–238 (1985) Google Scholar
  22. Sircar, S.: Separation of multi-component gas mixtures. U.S. Patent No 4,077,779 (1979) Google Scholar
  23. Sircar, S.: Separation of methane and carbon dioxide gas mixtures by pressure swing adsorption. Sep. Sci. Technol. 23, 519–529 (1988) CrossRefGoogle Scholar
  24. Sircar, S., Golden, C.M.A.: PSA process for removal of bulk CO2 from a wet high temperature gas. U.S. Patent No 6,322,612 (2001) Google Scholar
  25. Sircar, S., Kratz, W.C.: Simultaneous production of hydrogen and carbon dioxide from steam reformer off-gas by pressure swing adsorption. Sep. Sci. Technol. 23, 2397–2415 (1988) CrossRefGoogle Scholar
  26. Sircar, S., Kumar, R., Anselmo, K.J.: Effects of column non-isothermality or non-adiabaticity on the adsorption breakthrough curves. Ind. Eng. Chem. Proc. Des. Dev. 22, 10–15 (1983) CrossRefGoogle Scholar
  27. Sircar, S., Hufton, J.R., Nataraj, S.: Process and apparatus for the production of hydrogen by steam reforming of hydrocarbon. U.S. Patent No 6,103,143 (2000) Google Scholar
  28. Stiegel, G.J., Ramezan, M.: An overview of the U.S. Department of Energy’s gasification technology program. ACS Symp. Div. Fuel Chem. 48, 402–404 (2003) Google Scholar
  29. Viaswinkel, E.E., Posthuma, S.A., Zuideveld, P.L.: The Shell gasification technology offers clean solutions for refineries and utility companies. Inst. Chem. Eng. Symp. Ser. 143, 81–90 (1997) Google Scholar
  30. Waldron, W.E., Hufton, J.R., Sircar, S.: Production of hydrogen by cyclic sorption enhanced reaction process. AIChE J. 47, 1477–1479 (2001) CrossRefGoogle Scholar
  31. Xu, J.G., Froment, G.F.: Methane steam reforming, methanation, and water gas shift: I. Intrinsic kinetics. AIChE J. 35, 88–96 (1989) CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC 2007

Authors and Affiliations

  • K. B. Lee
    • 1
  • M. G. Beaver
    • 1
  • H. S. Caram
    • 1
  • S. Sircar
    • 1
  1. 1.Chemical Engineering DepartmentLehigh UniversityBethlehemUSA

Personalised recommendations